ChemCatChem
·
2022
·Vol. 14
·期 6
·e202101765
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IF 5.497
Jingkun Wang,Chengqiang Wang,Yanhui Song,Wenbo Sha,Zhiyuan Wang,Hailiang Cao,Min Zhao,Peizhi Liu,Junjie Guo
Graphical In this article, the synergy effect of active edge sites engineering of antimonene to expose more active sites and surface modulation strategy by ionic liquid to facilitate the electron transfer are adopted to endows AMNDs the boosted electrocatalytic activity toward HER in alkaline media. Ionic liquid modified active edge-rich AMNDs revealed absorbing activity towards the HER, such as a small overpotential of 116 mV at 10 mA cm −2 , a Tafel slope of 104 mV dec −1 and a long-term stability. Manipulating the size and surface modulation strategy provides a simple way for designing low-cost and high-efficiency electrocatalytic materials. Two-dimensional (2D) monoelemental antimonene has aroused great research interest since it emerged as a promising electrocatalyst for the hydrogen evolution reaction (HER). Nevertheless, the catalytic efficiency of the reported antimonene catalysts has been limited by their poor conductivity and low-density of exposed active sites. Herein, the active edge sites engineering is adopted to expose abundant catalytically active edge sites by decreasing the size of antimonene nanosheets to ultrasmall-sized antimonene nanodots (AMNDs). Meanwhile, the synergy effect of the surface modulation strategy by decorating the base surface of AMNDs using the ionic liquid benefits the mass transfer during the HER process. Impressively, the ionic liquid modified AMNDs (noted as IL-AMNDs) achieve a low overpotential of 116 mV at the current density of 10 mA cm −2 and excellent long-term durability, even superior to many other previously reported 2D catalysts. This work spreads the way out for the development of highly active and efficient hydrogen production catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yaxing Li,Rui Zhang,Xianghai Meng,Ping Ouyang,Haiyan Liu,Chunming Xu,Zhichang Liu
Acid-soluble oil (ASO) was produced during isobutane alkylation catalyzed by chloroaluminate ionic liquids (CAILs). However, the ASO composition characterizations and deactivated CAIL regeneration pathway were not clarified. In this work, a series of characterizations (elemental analysis and infrared, ultraviolet, and mass spectroscopy) were performed to reveal the ASO composition. The result showed that ASO contained numerous conjugated cycloolefins with various alkyl substituents and a few O1–O5 compounds. The activity index (AI) value of fresh CAILs was 1.74 and decreased to 1.18 with the addition of 9.09 wt % ASO because the [Al2Cl7]− anion in CAILs was complexed by C═C and C═O bonds in ASO. The hydrogenation regeneration of deactivated CAILs on the Pd/C catalyst was studied. The AI value of regenerated CAILs increased to 1.45 because unsaturated bonds in ASO were hydrogenated to saturation. Recovery of unsaturated hydrocarbons followed the order benzene > 1-methylcyclopentene > pentamethylcyclopentadiene. This work demonstrated that low ASO recovery was attributed to the partial occupation of the π-electron of unsaturated bonds by the [Al2Cl7]− anion.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Bing Liu,Yongzhong Jia,Zezheng Zhang,Huaxin Sun,Ying Yao,Yan Jing,Mixiang Qi,Quanyou Zhang
The solvent extraction separation of lithium isotopes has become of growing interest due to the need for 6 Li and 7 Li isotopes in the nuclear industry. A one-step synthesis of room temperature ionic liquid with low viscosity 1-Ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIm][NTf 2 ]) (with reaction yields of 87.47%) was used by the ultrasonic method. The addition of ionic liquid [EMIm][NTf 2 ] in the system significantly improved the extraction efficiency and separation factor compared to the traditional organic solvent anisole for extraction separation of lithium isotopes. The distribution ratio increased from 0.00145 (with the single stage separation factor of 1.024 ± 0.001) to 0.134 (with the single stage separation factor of 1.034 ± 0.001). Furthermore, a multi-stage extraction process was intended to enhance lithium isotope separation performance. Each stage of stripping can be considered as an extraction separation equilibrium process, in which the strip liquor from the load organic phase is used for separation in the next stage as the “original aqueous solution”. The abundance of 6 Li + gradually improved with an increase in the extraction stages. The relative abundance of 6 Li + increased by 1.492% at the 20-stage extraction separation (from 7.53% to 9.022%). This new and simple approach (stripping cross-flow multistage method (SCFM)) was to achieve large enrichment of lighter isotopes of lithium ( 6 Li + ) by combined extraction and stripping process. In summary, the present study offers the possibility for the enrichment of 6 Li + during lithium isotope extraction separation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yiru Gao,Yanan Hao,Wenxin Zhang,Yanan Wei,Yang Shu,Jianhua Wang
Phototherapy still lacks effectiveness in treating tissue infections due to poor penetration depth of light and laser-induced non-specific thermal diffusion. Microwave thermal therapy (MWTT) is advantageous as characterized by strong tissue penetration, and higher heating rate. In addition, transdermal delivery of drugs helps in the treatment of tissue infections. Herein, we present an all-in-one MW-therapeutic hydrogel for eradicating bacterial infections with transdermal drug delivery. A microwave-responsive ionic liquid (IL), i.e., vinylbenzyl trimethylammonium chloride (VBTMACl), and a transdermal-enhancer IL, i.e., [2-(methacryloyloxy)ethyl] trimethylammonium chloride (ChMACl), are copolymerized with acrylic acid (AA) to form the hydrogel VACPHs. Polyvinylpyrrolidone (PVP) is incorporated with VACPHs to improve their mechanical stability. The model drug levofloxacin (LEVO) is subsequently loaded into the hydrogel, and the VACPHs-LEVO shows strong antibacterial effect. It is attributed to the efficient microwaveocaloric therapy of VBTMACl and enhanced transdermal antibiotic delivery by ChMACl. The drug delivery hydrogel developed in this research exhibits excellent performance for the treatment of deep tissue infections.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2021
·
IF 2.262
Shanshan Dai,Minmin Tao,Hongsheng Lu
CO2-responsive wormlike micelles based on ionic liquid 1,1,3,3-tetramethylguanidine-oleic acid (TMG-OA) and cationic surfactant tetradecyl trimethyl ammonium bromide (TTAB) was designed in this work, avoiding the volatileness and flammability of traditional wormlike micelles formed with amines. It provides a new method of preparing CO2-switchable wormlike micelles based on ionic liquid with acidic group. The ionic liquid TMG-OA was prepared by the direct neutralization reaction between TMG and HOA at the molar ratio of 1:1. Due to the excellent stability and switchability demonstrated by thermogravimetry (TGA) and pH, TMG-OA can be treated as nonvolatile surfactant with CO2-responsive acidic group. Then the worm-based viscoelastic fluid is formed by the electrostatic interaction between TTAB and TMG-OA, and the steady and dynamic rheology show that the viscoelastic fluid has CO2-switchable thinning behavior. The switchable behavior is consistent with the reversible transition of microstructure from wormlike micelles to emulsion, which were detected by the dynamic light scattering (DLS) and cryo-transmission electron microscope (Cryo-TEM). The microstructural transition is induced by the reversible conversation between TMG-OA component and HOA component upon CO2 and N2/heat.
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Polymers
·
2021
·Vol. 13
·期 5
·742
·
IF 4.329
Wanyu Chen,Siyuan Liu,Le Guo,Guixia Zhang,Heng Zhang,Meng Cao,Lili Wu,Tianxing Xiang,Yong Peng
An ionic liquid-based ionically cross-linked gel polymer electrolyte (GPE-ILs) was successfully synthesized using acrylic acid, 2-diethylaminoethyl methacrylate, methyl methacrylate, and ionic liquids. Electrochromic devices (ECDs) with an architecture of glass/FTO/WO3/GPE-ILs/FTO/glass were fabricated by a laminating technology. The devices showed performances of large optical modulation of 49.9% at 650 nm, short switching times with the coloration time (tc) of 7 s and the bleaching time (tb) of 4 s, high coloration efficiency of 96.2 cm2C−1, and cycling stability of 200 cycles. The GPE-ILs exhibits high ionic conductivity, superior thermal stability and good self-healing ability. GPE-ILs demonstrates an ionic conductivity of 3.19 × 10−3S cm−1at 25 °C and the same ions migration behaviors with most widely used liquid electrolyte between −10 and 80 °C maintains more than 80% of its tensile strength after self-healing and received only 5% weight loss at 300 °C.Keywords:electrochromic device;ionically cross-linked gel;electrolyte;ionic liquids
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PubMed
高影响因子
ULTRASONICS SONOCHEMISTRY
·
2021
·
IF 7.491
Wenxue Zhang,Liurong Huang,Wenwen Chen,Jiale Wang,Shiheng Wang
In this work, the effect of dual-frequency ultrasound-assisted ionic liquids (ILs) pretreatment on the functional properties of soy protein isolate (SPI) hydrolysates was investigated. The degree of hydrolysis (DH) of SPI pretreated by ultrasound and [BMIM][PF 6 ] increased by 12.53% as compared to control ( P < 0.05). More peptides with low molecular weight were obtained, providing support for the changes in DH. The trichloroacetic acid-nitrogen soluble index presented an increase, suggesting a better protein hydrolysate property. The increase in the calcium-binding activity showed the ultrasound-assisted ILs pretreatment could potentially improve bone health. The foaming capacity and stability of SPI hydrolysates pretreated by ultrasound-assisted [BMIM][PF 6 ] always increased remarkably as compared to ultrasound-assisted [BDMIM][Cl] pretreatment. However, the synergistic effect of ultrasound-assisted [BMIM][PF 6 ] on the emulsifying activity and antioxidant activities (DPPH and hydroxyl radical scavenging activity) was not as ideal as ultrasound-assisted [BDMIM][Cl] pretreatment, which may be affected by the structure of peptide. In conclusion, these results indicated the combination of dual-frequency ultrasound and ionic liquids would be a promising method to improve the functional properties of SPI hydrolysates and broaden the application scope of compound modification in proteolysis industry.
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PubMed
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FUEL
·
2021
·
IF 6.609
Guojia Yu,Xiaojia Wu,Lu Wei,Zhiyong Zhou,Wei Liu,Fan Zhang,Yixin Qu,Zhongqi Ren
Ionic liquids (ILs) are highly efficient green solvents for the removal of thiophene sulfides. Several acidic ionic liquids (ILs) were synthesized with N-formylmorpholine (NFM) as cation and formic acid (HCOOH), sulfuric acid (H 2 SO 4 ), p-toluenesulfonic acid (Tos), trifluoroacetic acid (TFA) as anions. [NFM][TFA] was selected in one-pot extraction-oxidative desulfurization process. The initial sulfide concentrations, competition with olefins and aromatics and the desulfurization mechanism were explored. When V IL /V oil = 1:20, O/S = 3, 60 °C, the desulfurization efficiency of DMDBT and DBT were 99.82% and 99.67% in 30 min, respectively. After recycling five times, the desulfurization efficiency of [NFM][TFA] for DBT could maintain over 98%. When the initial real diesel concentration of 535 ppm and 298 ppm, the desulfurization efficiencies of real diesel were 44.42% and 56.46%, the values increased to 85.73% and 92.13% after extraction and re-extraction by [DBU][Pr]. The mechanism of desulfurization process was proposed that [NFM][TFA] reacted with H 2 O 2 to form corresponding peroxyacid transition state, and DBT in IL phase was oxidized to the corresponding sulfones.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 4
·1182-1193
·
IF 3.186
Shi Kaiyu,Guo Liying,Zheng Rongrong,Wang Haiyue,Chen Yanming
Five kinds of diacid comprising ionic liquid catalyst [HO 3 S–(CH 2 ) 4 -mim]Cl–MCl x ] were prepared, and their chemical structure, thermal stability and acidity were tested and analyzed. The performance evaluation of catalysts was carried out, and the process parameters were optimized. The cycling stability of the catalysts was investigated. Then, the catalytic degradation of polyethylene terephthalate (PET) was studied, and used mineral water bottles as an example. The chemical structure and molecular weight of the degradation product terephthalic acid bis(2-hydroxyethyl) ester (BHET) were analyzed. The results showed that among the catalysts synthesized, [HO 3 S–(CH 2 ) 4 -mim]Cl–FeCl 3 had the great catalytic performance and good thermal stability. According to the thermal gravimeter analysis, the decomposition temperature of the diacid ionic liquid catalyst ranges from 400 to 560 °C, while the degradation reaction temperatures in this paper are all below 250 °C, so that it has good thermal stability. At 190 °C, the PET alcoholysis rate reached 98.7% and the BHET yield reached 95.5% for 6 h, and the highest catalytic activity could still be maintained after 6 cycles, which indicate that the catalyst has excellent performance for degrading PET, and will have a great application prospect. Graphic Abstract
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Liu Fan,Baohua Xu,Jie Li,Ruiyi Yan,Yanyan Diao,Chunshan Li
Diethylamine acetate as an ionic liquid is used as a catalyst for the Mannich reaction of propanal and formaldehyde to produce methacrolein. However, catalyst deactivation remains a serious problem that has not been studied. Here, the reaction was carried out using different temperatures, atmospheres, and reagents to probe the catalyst deactivation mechanism. The proposed mechanism was further supported by data from Fourier transform infrared and electrospray ionization tandem mass spectrometry. Based on this mechanism, kinetic study of catalyst deactivation reaction between diethylamine acetate and formaldehyde was conducted in its initial stage at 85–115 °C for 15–60 min, in order to avoid complex situations in the subsequent reaction. Moreover, the kinetics of diethylamine acetate-catalyzed Mannich reaction was examined, and the pre-exponential factor, activation energy, and reaction order of each reactant were calculated by regression. These results contribute to the industrial application of this catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Jun Shang,Yanni Guo,Deliang He,Wei Qu,Yining Tang,Lei Zhou,Rilong Zhu
A novel graphene oxide-dicationic ionic liquid composite (GO-DIL) was prepared by modifying graphene oxide (GO) with a dicationic ionic liquid (DIL), 3,3′-(butane-1,4-diyl) bis (1-methyl-1H-imidazol-3-ium) chloride ([C 4 (MIM) 2 ]Cl 2 ). GO and GO-DIL were characterized by SEM, BET, FTIR, and XPS, and the materials were used for Cr(VI) adsorption. Batch adsorption studies showed that adsorption reached equilibrium within 40 min, and the optimal pH was 3, where the electrostatic attraction between GO-DIL and Cr(VI) was maximized. The maximum theoretical Cr(VI) adsorption capacity ( q m ) was 271.08 mg g −1 , and q m remained above 228.00 mg g −1 after five cycles. The adsorption data were fitted well by both the pseudo-first-order kinetic model and the Langmuir model. Furthermore, thermodynamics calculations revealed that adsorption was a spontaneous endothermic process. Importantly, electrostatic attraction between Cr(VI) and the protonated imidazole N + of GO-DIL played a critical role in Cr(VI) adsorption, and Cr(VI) was reduced to Cr(III). Thus, GO-DIL is predicted to be an effective adsorbent for Cr(VI) and other heavy metal ions in wastewater.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Minzhi Du,Xinyi Chen,Kun Zhang
Ionic liquids (ILs) have been reported to modulate the thermoelectric properties of conducting polymers. However, there is still a lack of comprehensive understanding of the effects of ILs on their thermoelectric transport. Herein, we selected 1-ethyl-3-methylimidazolium dicyanamide (EMIM:DCA) to post-treat free-standing PEDOT nanowire (NW) films and the effects on thermoelectric performance were fully explored. EMIM:DCA post-treatment simultaneously increases the Seebeck coefficient (87% increment) and electrical conductivity (24% increment) of PEDOT NWs, resulting in an optimal power factor of 83.8 μW m–1 K–2 at room temperature. It demonstrates the first ever-reported free-standing IL/polymer composites and outperforms the majority of all IL/polymer composites. Based on experimental characterizations, we elucidate that IL-induced dedoping and the Soret effect synchronously determine the Seebeck coefficient enhancement, where the Soret effect plays a dominant role, accounting for 79.9% for PEDOT NW films with 80 wt % EMIM:DCA. By means of X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), and X-ray diffraction (XRD), we further confirm that IL-induced dedoping contributes to phase segregation and compact stacking of PEDOT chains, resulting in lowered carrier concentration for the enhanced Seebeck coefficient and facilitating carrier transport for higher electrical conductivity. More importantly, through Kang–Snyder transport modeling, we first find that the improved transport coefficient (σE0) by IL-induced dedoping also contributes to the Seebeck coefficient enhancement, shedding light on the mechanism that can be adopted to design high-performance thermoelectric materials with conducting polymers.
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